Unveiling the Antiferromagnetic Properties of CrPb (n = 3-20) Clusters.

Assembling antiferromagnetic (AFM) clusters is perhaps an effective way to construct AFM materials to meet the increasing demand for micro/nano spintronic devices, which promotes the exploration of AFM clusters. Herein, we unveil the structural evolution, electronic, and AFM properties of CrPb (n = 3-20) clusters based on density functional theory (DFT) calculations. It is found that the Cr impurities prefer the central axis positions of the skeleton in these CrPb (n = 3-20) clusters. For sizes n ≤ 6, their structures are exohedral structures with the two Cr atoms exposed outside, endohedral Cr@Pb configuration with one Cr atom interior appears at size 7, and the resulting endohedral structure is then gradually covered by the additional Pb atoms to form endohedral Cr@Pb structures for n = 15-20. All CrPb clusters are antiferromagnets, except for the ferrimagnetic CrPb with a net magnetic moment of 2 μ. The discovered stable CrPb cluster can assemble into dimers and trimers while maintaining its geometric structure and AFM properties, indicating the potential of becoming structural units for cluster-assembled AFM materials.